Dielectric properties of ultraviolet cured poly(dimethyl siloxane) sub-percolative composites containing percolative amounts of multi-walled carbon nanotubes

Abstract

In this study a new method of multi-walled carbon nanotube (MWCNT) incorporation was employed in the preparation of ultraviolet (UV) curable MWCNT-filled poly(dimethyl siloxane) (PDMS) composites. The composites were designed to contain amounts of MWCNT above the percolation threshold, without becoming conductive. Ultrasonicated and dispersed MWCNTs were co-precipitated together with an excess of short chain α,ω-vinyl terminated PDMS with a deficient amount of thiol-crosslinker and a photoinitiator (2,2-dimethoxy-2-phenylacetophenone, DMPA) into MeOH. The entire mixture was UV irradiated, resulting in a layer of hyperbranched PDMS forming around the MWCNTs. This MWCNT mixture was added to a hyperbranched long chain PDMS to provide concentrations of MWCNT of 0.33%, 0.66% and 1%, and a fully crosslinked system was obtained in a final photochemical curing. Rheology of the composites showed a moderate decrease in storage modulus (G′) across the entire frequency range in line with an increasing amount of MWCNT, thus demonstrating that the rheological percolation threshold was not reached throughout the concentration range. Dielectric spectroscopy measurements showed an increase in permittivity in line with an increasing MWCNT content as well as the desired frequency-dependent conductivity for all samples. The composites showed moderate dielectric breakdown strength of 48 V μm⁻¹ at 0.33 wt% MWCNT, which decreased throughout the samples to 20 V μm⁻¹ at 1 wt%. Temperature-dependent AC conductivity studies revealed that an increase in the sample temperature could explain the premature breakdown observed for those composites with higher MWCNT loading.